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<p>Layered organic–inorganic hybrid superlattices, with modular structural advantages, offer an interesting approach to overcome the challenges in modulating the efficiency of intersystem crossing (ISC). This hybrid material system integrates the variable electronic and atomic properties of inorganic metal layers with the programmable chemical properties of organic coordination layers, enabling regulation of electronic states, excitons and ISC processes. Here we demonstrate a precise ISC modulating strategy by constructing gold-based organic–inorganic layered hybrid superlattices, featuring alternately assembled atomically thin gold layers and 4-mercapto-benzamide-derived organic ligands layers. The confined layered structure achieves directional hybridization between transition metal <i>d</i> orbitals and delocalized electrons of organic moieties through controlled Au–<i>π</i> conjugation interactions. Femtosecond transient-absorption spectroscopy reveals that ISC time decreases from &gt;2 ps to 0.26 ps as interlayer spacing reduces, demonstrating the role of structural confinement in promoting ultrafast ISC. Moreover, temperature-dependent photoluminescence studies estimate the singlet–triplet energy gap at ∼20 meV, further supporting the enhanced ISC mechanism. This work introduces the design of hybrid superlattices with tailored spin–orbit interactions enabling tunable fluorescence and phosphorescence properties, paving the way for next-generation optoelectronic applications.</p><p></p>

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Layered hybrid superlattices with a regulated intersystem crossing process

  • 期刊论文

  • 发表日期：

    2025年11月13日

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  • Haosen Yang,
  • Yutong Zhang,
  • Zhengyao Qiu,
  • Hongfei Gu,
  • He Guo,
  • Tianqi Guo,
  • Pengfei Hu,
  • Lingyun Zhu,
  • Shuai Yue,
  • Xinfeng Liu,
  • Lin Guo

摘要

Layered organic–inorganic hybrid superlattices, with modular structural advantages, offer an interesting approach to overcome the challenges in modulating the efficiency of intersystem crossing (ISC). This hybrid material system integrates the variable electronic and atomic properties of inorganic metal layers with the programmable chemical properties of organic coordination layers, enabling regulation of electronic states, excitons and ISC processes. Here we demonstrate a precise ISC modulating strategy by constructing gold-based organic–inorganic layered hybrid superlattices, featuring alternately assembled atomically thin gold layers and 4-mercapto-benzamide-derived organic ligands layers. The confined layered structure achieves directional hybridization between transition metal d orbitals and delocalized electrons of organic moieties through controlled Au–π conjugation interactions. Femtosecond transient-absorption spectroscopy reveals that ISC time decreases from >2 ps to 0.26 ps as interlayer spacing reduces, demonstrating the role of structural confinement in promoting ultrafast ISC. Moreover, temperature-dependent photoluminescence studies estimate the singlet–triplet energy gap at ∼20 meV, further supporting the enhanced ISC mechanism. This work introduces the design of hybrid superlattices with tailored spin–orbit interactions enabling tunable fluorescence and phosphorescence properties, paving the way for next-generation optoelectronic applications.